Small molecules that self-assemble into well-ordered hierarchical superstructures direct the most complex tasks in biology. To create synthetic structures with similar functionality, chemists have employed noncovalent interactions to organize chromophores into large, well-defined structures, including systems that utilize both hydrogen-bonding (H-bonding) and π•••π interactions. Examples include homoaggregates, such as oligo(p-phenylenevinylenes) (OPVs) or substituted perylenediimides (PDI), where H-bonding precedes aggregation into π-stacked helices, or heteroaggregates that assemble into superstructures via multiple noncovalent interactions, such as a system consisting of either melamine or OPVs H-bonding with PDIs. In self-assembling systems where one-dimensional aggregates form, models have been developed to obtain association constants (Kas), thermodynamic parameters (ΔH° and ΔS°), and degrees of polymerization by attributing assembly to a single “dominant” noncovalent interaction. For heteroaggregation however, models that consider two or more components are rare and most simplify their description of assembly by only considering a single noncovalent interaction. This inability to model how different noncovalent recognition events work in concert to create superstructures limits the ability of scientists to create systems with the functional complexity found in natural systems.